Layered materials have been well investigated and have found widespread application because of their unique structures and properties. In this presentation, synthesis of various layered materials, particularly on the tailoring of their 3rd dimension, will be discussed, including (1) one-step direct synthesis of intercalated layered compounds; (2) one-step direct synthesis of colloidal single-layer nanosheets; (3) one-step direct synthesis of layered prisms. The applications of layered materials with various unique morphologies are also presented, including (a) layered intercalation compounds exhibiting negative swelling; (b) organic/inorganic hybrid nanocoatings with a nacre-like microstructure from one-step co-assembly, which possess exceptional mechanical, barrier, and flame retardant properties thanks to the high concentration (up to 70 wt%) of well-aligned inorganic nanosheets; (c) mechanochromic bi-layer hybrids with a high sensitivity and reversibility exhibiting vivid color change upon stretching; and (d) moisture responsive wrinkle dynamics inspired by human skin featuring different reversibility, stability, and thus versatile patterning. These multifunctional polymer based hybrids are promising for a wide range of applications such as packaging, anti-counterfeit tabs, encryption devices, water indicators, light diffusors, etc.